Proceedings of the National Academy of Sciences,
Год журнала:
2024,
Номер
121(51)
Опубликована: Дек. 13, 2024
Biomass-burning
organic
aerosol(s)
(BBOA)
are
rich
in
brown
carbon,
which
significantly
absorbs
solar
irradiation
and
potentially
accelerates
global
warming.
Despite
its
importance,
the
multiphase
photochemistry
of
BBOA
after
light
absorption
remains
poorly
understood
due
to
challenges
determining
oxidant
concentrations
reaction
kinetics
within
aerosol
particles.
In
this
study,
we
explored
photochemical
reactivity
particles
S(IV)
oxidation
sulfate.
We
found
that
sulfate
formation
under
is
predominantly
driven
by
photosensitization
involving
triplet
excited
states
(
3
*
)
instead
iron,
nitrate,
photochemistry.
Rates
three
orders
magnitude
higher
than
those
observed
bulk
solution,
primarily
fast
interfacial
reactions.
Our
results
highlight
chemistry
can
greatly
contribute
sulfate,
as
an
example
secondary
pollutants.
Photosensitization
will
likely
become
increasingly
crucial
intensified
wildfires.
Environmental Science & Technology,
Год журнала:
2024,
Номер
58(25), С. 11105 - 11117
Опубликована: Июнь 12, 2024
Volatile
chemical
products
(VCPs)
are
increasingly
recognized
as
significant
sources
of
volatile
organic
compounds
(VOCs)
in
urban
atmospheres,
potentially
serving
key
precursors
for
secondary
aerosol
(SOA)
formation.
This
study
investigates
the
formation
and
physicochemical
transformations
VCP-derived
SOA,
produced
through
ozonolysis
VOCs
evaporated
from
a
representative
room
deodorant
air
freshener,
focusing
on
effects
evaporation
its
molecular
composition,
light
absorption
properties,
reactive
oxygen
species
(ROS)
generation.
Following
evaporation,
solutes
become
concentrated,
accelerating
reactions
within
matrix
that
lead
to
42%
reduction
peroxide
content
noticeable
browning
SOA.
process
occurs
most
effectively
at
moderate
relative
humidity
(∼40%),
reaching
maximum
solute
concentration
before
solidification.
Molecular
characterization
reveals
evaporating
SOA
produces
highly
conjugated
nitrogen-containing
interactions
between
existing
or
transformed
carbonyl
reduced
nitrogen
species,
likely
acting
chromophores
responsible
observed
brownish
coloration.
Additionally,
reactivity
was
elucidated
heterogeneous
oxidation
sulfur
dioxide
(SO
Proceedings of the National Academy of Sciences,
Год журнала:
2024,
Номер
121(51)
Опубликована: Дек. 13, 2024
Biomass-burning
organic
aerosol(s)
(BBOA)
are
rich
in
brown
carbon,
which
significantly
absorbs
solar
irradiation
and
potentially
accelerates
global
warming.
Despite
its
importance,
the
multiphase
photochemistry
of
BBOA
after
light
absorption
remains
poorly
understood
due
to
challenges
determining
oxidant
concentrations
reaction
kinetics
within
aerosol
particles.
In
this
study,
we
explored
photochemical
reactivity
particles
S(IV)
oxidation
sulfate.
We
found
that
sulfate
formation
under
is
predominantly
driven
by
photosensitization
involving
triplet
excited
states
(
3
*
)
instead
iron,
nitrate,
photochemistry.
Rates
three
orders
magnitude
higher
than
those
observed
bulk
solution,
primarily
fast
interfacial
reactions.
Our
results
highlight
chemistry
can
greatly
contribute
sulfate,
as
an
example
secondary
pollutants.
Photosensitization
will
likely
become
increasingly
crucial
intensified
wildfires.